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<p>A series of graphene-modified copper–metal–organic framework composites (G-Cu-MOF-0.3, G-Cu-MOF-0.5, G-Cu-MOF-1) were fabricated via a solvothermal method. Structural characterizations verified that graphene was successfully composited without damaging the Cu-MOF crystalline framework, among the four materials, G-Cu-MOF-0.5 exhibits the largest specific surface area and pore size. Electrochemical results showed that G-Cu-MOF-0.5 displayed the best CO₂ electroreduction performance, with a current density of −&#xa0;11&#xa0;mA&#xa0;cm⁻², a double-layer capacitance (Cdl) of 4.97 mF&#xa0;cm⁻² and a Tafel slope value of 36.5 mV dec⁻¹. At −&#xa0;1.5&#xa0;V vs. RHE, the total Faradaic efficiency for CH₄ and CO reached 24% with stable operation over 12&#xa0;h. Graphene modification significantly improves the conductivity, active site density, and structural stability of Cu-MOF, realizing efficient and controllable CO<sub>2</sub> conversion to C1 products. The hydrogen evolution reaction (HER) remains the dominant side reaction, and the Faradaic efficiency toward CH<sub>4</sub> is still moderate, leaving room for further selectivity optimization.This work provides a feasible strategy for designing MOF–carbon composites for electrocatalytic CO₂ reduction to methane.</p>

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Tailoring of Graphene-Modified Cu-MOFs for Improved Controllable CO2 Electroreduction Toward CH4 Production

  • 期刊论文

  • 发表日期：

    2026年7月6日

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  • Haixia Wang,
  • Yilei Sun,
  • Chuang Liu,
  • Zeda D. Meng,
  • Won-Chun Oh

摘要

A series of graphene-modified copper–metal–organic framework composites (G-Cu-MOF-0.3, G-Cu-MOF-0.5, G-Cu-MOF-1) were fabricated via a solvothermal method. Structural characterizations verified that graphene was successfully composited without damaging the Cu-MOF crystalline framework, among the four materials, G-Cu-MOF-0.5 exhibits the largest specific surface area and pore size. Electrochemical results showed that G-Cu-MOF-0.5 displayed the best CO₂ electroreduction performance, with a current density of − 11 mA cm⁻², a double-layer capacitance (Cdl) of 4.97 mF cm⁻² and a Tafel slope value of 36.5 mV dec⁻¹. At − 1.5 V vs. RHE, the total Faradaic efficiency for CH₄ and CO reached 24% with stable operation over 12 h. Graphene modification significantly improves the conductivity, active site density, and structural stability of Cu-MOF, realizing efficient and controllable CO2 conversion to C1 products. The hydrogen evolution reaction (HER) remains the dominant side reaction, and the Faradaic efficiency toward CH4 is still moderate, leaving room for further selectivity optimization.This work provides a feasible strategy for designing MOF–carbon composites for electrocatalytic CO₂ reduction to methane.